Skip to main content

Advertisement

SpringerLink
Log in

Betulinol and wood sterols in sediments contaminated by pulp and paper mill effluents: dissolution and spatial distribution

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The goal was to determine dissolution potency of betulinol and wood sterols (WSs) from pulp and paper mill-contaminated sediments and the current stratification for assessment the load due to potential erosion in the river-like watercourse. Both compounds are wood extractives, which may be toxic to benthos and fish. This research continues a study in which other wood extractives, resin acids and their derivative, retene, were analysed. Sediments were collected from 1, 3.5, 12, 15, and 33 km downstream from the pulp and paper mills, and from 2 upstream reference sites. The dissolution potency into sediment–water elutriates (1 + 4 v/v) was studied by two agitation times and temperatures. The vertical amounts of extractives were determined from the uppermost 20 cm of sediment. The amounts of extractives potentially released were estimated from the sediment layers 0–2 and 2–5 cm by using spatial interpolation. According to the interpolation, the total amount of betulinol and β-sitosterol was calculated as kg/ha in the whole sediment area. Significant concentrations of betulinol (1,666 μg/g, dw) and WSs (2,886 μg/g, dw) were measured from the sediments. According spatial interpolation, the highest calculated amount of betulinol (4,726 kg/ha) and that of the most abundant WS, β-sitosterol (3,571 kg/ha), were in the lake where the effluents were discharged. In the dissolution experiment, the highest concentration of betulinol in sediment (0–10 cm) and elutriate was 412 μg/g (dw) and 165 μg/l, respectively. For WSs, concentrations were 768 μg/g (dw) in sediment and 273 μg/l in elutriate. In a worst-case scenario, betulinol may be desorbed to water in concentrations which are hazardous to aquatic animals. Instead WSs are not a risk in this study area. The amount of desorption varied depending on the concentration of contaminants in sediment, the nature of disturbance, and the sediment organic carbon content.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4

Similar content being viewed by others

References

  • Abyshev AZ, Agaev EM, Guseinov AB (2007) Studies of the chemical composition of birch bark extracts (Cortex betula) from the Betulaceae family. Pharm Chem J 41:419–423

    Article  CAS  Google Scholar 

  • Ali M, Sreekrishnan TR (2001) Aquatic toxicity from pulp and paper mill effluents: a review. Adv Environ Res 5:175–196

    Article  CAS  Google Scholar 

  • Anonymous (1981) Äänekoski-Vaajakoski vesireitin velvoitetarkkailu v. 1981. Metsäliiton teollisuus oy, Äänekosken tehtaat, Keski-Suomen selluloosa oy, Kemira oy, Vihtavuoren tehtaat, Suolahden kaupunki, Laukaan kunta, Äänekosken kaupunki (in Finnish)

  • Anonymous (2006a) Oy Metsä-Botnia Ab:n sellutehtaan ja Oy Polargas Ab:n happilaitoksen ympäristölupa, Äänekoski. Itä-Suomen ympäristölupavirasto, ISY-2004-Y-259 (in Finnish)

  • Anonymous (2006b) Finnforest Oyj ympäristölupa, Suolahti. Keski-Suomen ympäristökeskus, KSU-2004-Y-370/111 (in Finnish)

  • Anonymous (2006c) Äänekosken metsäteollisuusintegraatin jäteveden-puhdistamon ympäristölupa, Äänekoski. Itä-Suomen ympäristölupavirasto, ISY-2004-Y-258 (in Finnish)

  • Anonymous (2007) Botnia vuosiraportti 2007. http://www.metsafibre.fi/Uutiset/Material%20Archive/Botnia_vsk_2007.pdf. Accessed 28 June 2012 (in Finnish)

  • Anonymous (2011a) EMAS ympäristöselonteko 2006–2008, Keskeiset tiedot ympäristövaikutuksista ja ympäristönsuojelun tason kehittymisestä, M-real Äänekoski Paper. http://ec.europa.eu/environment/emas/pdf/es_library/21_fi_m-real_aanekoski_06-fi.pdf. Accessed 28 June 2012 (in Finnish)

  • Anonymous (2011b) Discharge rates collected from the website of the Finland’s environmental administration: www.ymparisto.fi. Accessed 28 June 2012 (in Finnish)

  • Ayebo A, Breuer GM, Cain TG, Wichman MD, Subramanian P, Reynolds SJ (2006) Sterols as bio-markers for waste impact and source characterization in stream sediment. J Environ Health 68:46–50

    CAS  Google Scholar 

  • Baborowski M, von Tuempling W, Friese K (2004) Behaviour of suspended particulate matter (SPM) and selected trace metals during the 2002 summer flood in the River Elbe (Germany) at Magdeburg monitoring station. Hydrol Earth Syst Sc 8:135–150

    Article  CAS  Google Scholar 

  • Billiard SM, Querbach K, Hodson P (1999) Toxicity of retene to early life stages of two freshwater fish species. Environ Toxicol Chem 18:2070–2077

    Article  CAS  Google Scholar 

  • Chan K-H, Lam MHW, Poon K-F, Yeung H-Y, Chiu TKT (1998) Application of sedimentary fecal stanols and sterols in tracing sewage pollution in coastal waters. Water Res 32:225–235

    Article  CAS  Google Scholar 

  • Chen W, Kan AT, Fu G, Vignona LC, Tomson MB (1999) Adsorption-desorption behaviors of hydrophobic organic compounds in sediments of Lake Charles, Louisiana, USA. Environ Toxicol Chem 18:1610–1616

    Google Scholar 

  • Christianson-Heiska I, Wahteristo P, Kastilan E-L, Bergelin E, Bylund G, Isomaa B (2004) Effects of the wood extractive betulinol and 17β-oestradiol on reproduction in zebrafish, Danio rerio (Hamilton) — complications due to bacterial infection. J Fish Dis 27:267–276

    Article  CAS  Google Scholar 

  • Christianson-Heiska IL, Haavisto T, Paranko J, Bergelin E, Isomaa B (2008) Effects of the wood extractives dehydroabietic acid and betulinol on reproductive physiology of zebrafish (Danio rerio) — a two-generation study. Aquat Toxicol 86:388–396

    Article  CAS  Google Scholar 

  • Fujioka T, Kashiwada Y, Kilkuskie RE, Cosentino LM, Ballas LM, Jiang JB, Janzen WP, Chen I-S, Lee K-H (1994) Anti-AIDS agents, 11. Betulinic acid and platanic acid as anti-HIV principles from Syzigium claviflorum, and the anti-HIV activity of structurally related triterpenoids. J Nat Prod 57:243–247

    Article  CAS  Google Scholar 

  • Förstner U, Heise S, Schwartz R, Westrich B, Ahlf W (2004) Historical contaminated sediments and soils at the river basin scale. Examples from the elbe river catchment area. J Soils Sediments 4:247–260

    Article  Google Scholar 

  • Granberg K, Hynynen J, Meriläinen J, Mäkelä H, Palomäki A, Bibiceanu S (1987) Äänekoski-Vaajakoski vesireitin velvoitetarkkailu vuonna 1986. Institute of Environmental Research of Jyväskylä (in Finnish)

  • Hickey CW, Martin ML (1995) Relative sensitivity of five benthic invertebrate species to reference toxicants and resin-acid contaminated sediments. Environ Toxicol Chem 14:1401–1409

    Article  CAS  Google Scholar 

  • Hilscherova K, Dusek L, Kubik V, Cupr P, Hofman J, Klanova J, Holoubek I (2007) Redistribution of organic pollutants in river sediments and alluvial soils related to major floods. J Soils Sediments 7:167–177

    Article  CAS  Google Scholar 

  • Hollert H, Dürr M, Haag I, Wölz J, Hilscherova K, Blaha L, Gerbersdorf SU (2007) Influence of hydrodynamics on sediment ecotoxicity. In: Westrich B, Förstner U (eds) Sediment dynamics and pollutant mobility in rivers. Springer, Berlin, Germany, pp 401–416

    Google Scholar 

  • Hutchins FE (1979) Toxicity of pulp and paper mill effluent: a literature review. Western Fish Toxicology Station, U.S. Environmental Protection Agency

  • Hynynen J, Palomäki A, Meriläinen JJ, Witick A, Mäntykoski K (2004) Pollution history and recovery of a boreal lake exposed to a heavy bleached pulping effluent load. J Paleolimnol 32:351–374

    Article  Google Scholar 

  • IPCC (2007) Climate Change 2007: Synthesis report. Contribution of working groups I, II and III to the Fourth Assessment Report of the Intergovernmental Panel on Climate change. In Pachauri RK, Reisinger A (eds.) IPCC, Geneva, Switzerland

  • Jenkins RL, Wilson EM, Angus RA, Howell WM, Kirk M (2003) Androstenedione and progesterone in the sediment of a river receiving paper mill effluent. Toxicol Sci 73:53–59

    Article  CAS  Google Scholar 

  • Kaplin C, Hemming J, Holmblom B (1997) Improved water quality by process renewal in a pulp and paper mill. Boreal Env Res 2:239–246

    CAS  Google Scholar 

  • Karels A, Oikari A (2000) Effect of pulp and paper mill effluents on the reproductive and physiological status of perch (Perca fluviatilis L.) and roach (Rutilus rutilus L.) during the spawning period. Annls Zool Fennici 37:65–77

    Google Scholar 

  • Koistinen J, Lehtonen M, Tukia K, Soimasuo M, Lahtiperä M, Oikari A (1998) Identification of lipophilic pollutants discharged from a Finnish pulp and paper mills. Chemosphere 37:219–235

    Article  CAS  Google Scholar 

  • Kostamo A, Holmbom B, Kukkonen JVK (2004) Fate of wood extractives in wastewater treatment plants at kraft pulp mills and mechanical pulp mills. Water Res 38:972–982

    Article  CAS  Google Scholar 

  • Lahdelma I, Oikari A (2005) Resin acids and retene in sediments adjacent to pulp and paper industries. J Soils Sediments 5:74–81

    Article  CAS  Google Scholar 

  • Lahdelma I, Oikari A (2006) Stratigraphy of wood-derived sterols in sediments historically contaminated by pulp and paper mill effluents. J Paleolimnol 35:323–334

    Article  Google Scholar 

  • Lebo JA, Huckins JN, Petty JD, Cranor WL, Ho KT (2003) Comparisons of coarse and fine versions of two carbons for reducing the bioavailabilities of sediment-bound hydrophobic organic contaminants. Chemosphere 50:1309–1317

    Article  CAS  Google Scholar 

  • Lehtinen K-J, Mattsson K, Tana J, Engstrom C, Lerche O, Hemming J (1999) Effects of wood-related sterols on the reproduction, egg survival, and offspring of brown trout (Salmo trutta lacustris L.). Ecotoxicol Environ Saf 42:40–49

    Article  CAS  Google Scholar 

  • Leppänen H, Oikari AOJ (1999) Occurrence of retene and resin acids in sediments and fish bile from a lake receiving pulp and paper mill effluents. Environ Toxicol Chem 18:1498–1505

    Article  Google Scholar 

  • Leppänen H, Oikari A (2001) Retene and resin acid concentrations in sediment profiles of a lake recovering from exposure to pulp mill effluents. J Paleolimnol 25:367–374

    Article  Google Scholar 

  • Maatela P, Paasivirta J, Särkkä J, Paukku R (1990) Organic chlorine compounds in lake sediments.II Organically bound chlorine. Chemosphere 21:1343–1354

    Article  CAS  Google Scholar 

  • Makris SP, Banerjee S (2002) Fate of resin acids in pulp mill secondary treatment systems. Water Res 36:2878–2882

    Article  CAS  Google Scholar 

  • Mattson K, Lehtinen K-J, Tana J, Härdig J, Kukkonen J, Nakari T, Engström C (2001) Effects of pulp mill effluents and restricted diet on growth physiology of rainbow trout (Oncorhynchus mykiss). Ecotox Environ Safe 49:144–154

    Google Scholar 

  • Mellanen P, Petänen T, Lehtimäki J, Mäkelä S, Bylund G, Holbom B, Mannila E, Oikari A, Santti R (1996) Wood-derived estrogens: studies in vitro with breast cancer cell lines and in vivo in trout. Toxicol Appl Pharmacol 1136:381–388

    Article  Google Scholar 

  • Meriläinen P, Lahdelma I, Oikari L, Hyötyläinen T, Oikari A (2006) Dissolution of resin acids, retene and wood sterols from contaminated lake sediments. Chemosphere 65:840–846

    Article  Google Scholar 

  • Meriläinen PS, Krasnov A, Oikari A (2007) Time and concentration-dependent metabolic and genomic responses to exposure to resin acids in brown trout (Salmo trutta m. lacustris). Environ Toxicol Chem 26:1827–1835

    Article  Google Scholar 

  • Meriläinen P, Oikari A (2008) Uptake of organic xenobiotics by benthic invertebrates from sediment contaminated by the pulp and paper industry. Water Res 42:1715–1725

    Article  Google Scholar 

  • Moghaddam MG, Ahmad FBH, Samzadeh-Kermani A (2012) Biological activity of betulinic acid: a review. Pharmacology & Pharmacy 3:119–123

    Article  CAS  Google Scholar 

  • Nikkilä A, Kukkonen JVK, Oikari A (2001) Bioavailability of sediment-associated retene to an Oligohaete Lumbriculuc variegatus, effects of sediment organic carbon and retene concentrations. J Soils Sediments 1:137–145

    Article  Google Scholar 

  • Oikari A, Lönn B-E, Castrén M, Nakari T, Snickars-Nikinmaa B, Bister H, Virtanen E (1983) Toxicological effects of dehydroabietic acid (DHAA) on the trout, Salmo gairdneri Richardson, in fresh water. Water Res 17:81–89

    Article  CAS  Google Scholar 

  • Orrego R, Guchardi J, Beyger L, Krause R, Holdway D (2011) Comparative embryotoxicity of pulp mill extracts in rainbow trout (Oncorhynchus mykiss), American flagfish (Jordanella floridae) and Japanese medaka (Oryzias latipes). Aquat Toxicol 104:299–307

    Article  CAS  Google Scholar 

  • Owens JW (1991) The hazard assessment of pulp and paper effluents in the aquatic environment: a review. Environ Toxicol Chem 10:1511–1540

    Article  CAS  Google Scholar 

  • Palomäki A, Salo H (2008) Äänekoski-Vaajakoski vesireitin yhteistarkkailu vuonna 2007. Jyväskylän yliopiston ympäristöntutkimuskeskus, Tutkimusraportti 80/2008, Jyväskylä (in Finnish)

  • Park SS, Ertsfeld KM (1999) The effect of sediment organic carbon content on bioavailability of hydrophobic compounds in aquatic ecosystems. Environ Pollut 105:9–15

    Article  CAS  Google Scholar 

  • Peng G, Roberts JC (2000) Solubility and toxicity of resin acids. Wat Res 34:2779–2785

    Article  CAS  Google Scholar 

  • Pokhrel D, Viraraghavan T (2004) Treatment of pulp and paper mill wastewater — a review. Sci Total Environ 333:37–58

    Article  CAS  Google Scholar 

  • Rogers IH (1978) Environmental effects of terpenoid chemicals: a review. J Am Oil Chem Soc 55:A113–A118

    Article  Google Scholar 

  • Rämänen H (2008) History and ecotoxicological risk assessment of wood extractives in sediments contaminated by pulp and paper industry. Master of Science Thesis, University of Jyväskylä (in Finnish)

  • Rämänen H, Lassila H, Lensu A, Lahti M, Oikari A (2010) Dissolution and spatial distribution of resin acids and retene in sediments contaminated by pulp and paper industry. J Soils Sediments 10:349–358

    Article  Google Scholar 

  • Salina O, Alakurtti S, Pohjala L, Siiskonen A, Maass V, Maass M, Yli-Kauhaluoma J, Vuorela P (2010) Inhibitory effect of the natural product betulin and its derivatives against the intracellular bacterium Chlamydia pneumonia. Biochem Pharmacol 80:1141–1151

    Article  Google Scholar 

  • Saski EK, Mikkola R, Kukkonen JVK, Salkinoja-Salonen MS (1997) Bleached kraft pulp mill discharged organic matter in recipient lake sediment. Environ Sci Pollut Res 4:194–202

    Article  CAS  Google Scholar 

  • Sjöström E (1993) Wood chemistry — fundamentals and applications, 2nd edn. Acad. Press (Ltd.), San Diego

    Google Scholar 

  • Stachel B, Goetz R, Herrmann T, Krueger F, Knoth W, Paepke O, Rauhut U, Reincke H, Schwartz R, Steeg E, Uhlig S (2004) The Elbe flood in August 2002 — Occurrence of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans (PCDD/F) and dioxin-like PCB in suspended particulate matter (SPM), sediment and fish. Water Sci Technol 50:309–316

    CAS  Google Scholar 

  • Suntio LR, Shiu WY, Mackay D (1988) A review of the nature and properties of chemicals present in pulp mill effluents. Chemosphere 17:1249–1290

    Article  CAS  Google Scholar 

  • Tremblay L, van der Kraak G (1998) Use of a series of homologous in vitro and in vivo assays to evaluate the endocrine modulating actions of beta-sitosterol in rainbow trout. Aquat Toxicol 43:149–162

    Article  CAS  Google Scholar 

  • Tremblay L, van der Kraak G (1999) Comparison between the effects of the phytosterol β-itosterol and pulp and paper mill effluents on sexually immature rainbow trout. Environ Toxicol Chem 18:329–336

    Article  CAS  Google Scholar 

  • Tuuri A, Valmunen PM, Nuikki P, Klementti K, Steffa T, Mason P (1996) Äänekoski Mills 1886–1996. Metsä-Serla Oy, F.G. Lönnberg, Helsinki, Finland

  • Vehniäinen E-R, Häkkinen J, Oikari A (2003) Photoinduced lethal and sublethal toxicity of retene, a polycyclic aromatic hydrocarbon derived from resin acid, to coregonid larvae. Environ Toxicol Chem 22:2995–3000

    Article  Google Scholar 

  • Vikström F, Holmbom B, Hamunen A (2005) Sterols and triterpenyl alcohols in common pulpwoods and black liquor soaps. Holz als Roh- und Werkstoff 63:303–308

    Article  Google Scholar 

  • Westrich B, Li C-C, Hammer D, Förstner U (2007) Requirement on sediment data quality — hydrodynamics and pollutant mobility in rivers. In: Westrich B, Förstner U (eds) Sediment dynamics and pollutant mobility in rivers. Springer, Berlin, Germany, pp 49–65

    Chapter  Google Scholar 

Download references

Acknowledgements

We would like to show our appreciation to the University of Jyväskylä and the Academy of Finland for financing this project (7109823 to A.O.). In addition, we wish to thank Marja Lahti for informational help as well as Mervi Koistinen and Leena Siitonen for their technical assistance.

Author information

Authors and Affiliations

  1. Department of Biological and Environmental Sciences, Division of Environmental Science and Technology, University of Jyväskylä, 40014, Jyväskylä, Finland

    H. Ratia, H. Rämänen, A. Lensu & A. Oikari

Authors
  1. H. Ratia
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. H. Rämänen
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. A. Lensu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. A. Oikari
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to H. Ratia.

Additional information

Responsible editor: Leif Kronberg

Equal contribution as the first author: Heli Ratia and Heli Rämänen

Rights and permissions

Reprints and permissions

About this article

Cite this article

Ratia, H., Rämänen, H., Lensu, A. et al. Betulinol and wood sterols in sediments contaminated by pulp and paper mill effluents: dissolution and spatial distribution. Environ Sci Pollut Res 20, 4562–4573 (2013). https://doi.org/10.1007/s11356-012-1381-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-012-1381-3

Keywords

Search

Navigation